CN102836638A - Process for removing NOx from smoke by two-stage reduction coupling complexation absorption with magnetic biological microspheres - Google Patents
Process for removing NOx from smoke by two-stage reduction coupling complexation absorption with magnetic biological microspheres Download PDFInfo
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- CN102836638A CN102836638A CN2012102764025A CN201210276402A CN102836638A CN 102836638 A CN102836638 A CN 102836638A CN 2012102764025 A CN2012102764025 A CN 2012102764025A CN 201210276402 A CN201210276402 A CN 201210276402A CN 102836638 A CN102836638 A CN 102836638A
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- Y—GENERAL TAGGING OF NEW TECHNOLOGICAL DEVELOPMENTS; GENERAL TAGGING OF CROSS-SECTIONAL TECHNOLOGIES SPANNING OVER SEVERAL SECTIONS OF THE IPC; TECHNICAL SUBJECTS COVERED BY FORMER USPC CROSS-REFERENCE ART COLLECTIONS [XRACs] AND DIGESTS
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Abstract
The invention provides a process for removing NOx from smoke by two-stage coupling complexation absorption with magnetic biological microspheres. The process comprises the steps of separately immobilizing two domesticated reducing bacteria by using magnetic chitosan microspheres as immobilizing vectors; filling in a first stage reducing regeneration tower and a second stage reducing regeneration tower respectively; performing a complexing absorption of a simulated smoke containing NOx in an absorption tower through FeII(EDTA); contacting an absorption solution after the complexing absorption of NOx with FeII(EDTA)NO reducing bacterium immobilizing microspheres in the first stage reducing regeneration tower, to reduce FeII(EDTA)NO to N2; and then contacting the absorption solution after the complexing absorption of NOx with FeIII(EDTA) reducing bacterium immobilizing microspheres in the second stage reducing regeneration tower, to reduce FeIII(EDTA)NO to FeII(EDTA); so that the complexing absorption solution can be regenerated. The process can improve density of preponderant bacteria in a system, keeps the performance of the preponderant bacteria stable, overcomes substrate competitive inhibition problems among components in the absorption solution, and is helpful for increasing biological reduction rate.
Description
[technical field]
The present invention relates to the gas denitrifying technology field, be specifically related to a kind of magnetic bio microballoon two-stage reductive coupling complexed absorption and remove NO in the flue gas
xTechnology.
[background technology]
Nitrogen oxide (NO
x) be the one of the main reasons that causes atmosphere pollution accidents such as acid rain, photochemical fog, serious to harm such as human body, ecological environments.Along with the quick increase of its discharge capacity and people environmental quality requirement improved constantly NO in recent years
xThe pollution problem that causes more and more comes into one's own.A large amount of fume emissions of fossil-fuel-fired generation are NO
xGet into the main path of environment, because smoke discharge amount is big, and NO wherein
xThe solubility of main component nitric oxide (NO accounts for 95%) in water very low, intractability is bigger.At present, only have in the world with NH
3For the SCR (SCR) and the SNCR (SNCR) of reducing agent obtained commercial Application to a certain degree, but still there is high, the NH of investment operating cost in these two kinds of methods
3Leak, produce defectives such as secondary pollution, the easy inefficacy of catalyst.Thereby developing new gas denitrifying technology has become one of current environment protection hot research fields.
The complexed absorption method is a kind of flue-gas denitrification method that grows up the beginning of the seventies in last century, has obtained more deep research in states such as Holland, the U.S., Japan.It is to utilize the liquid complexing absorbent (like Fe
II(EDTA)) thus it is changed the rapid complexing of the NO in the flue gas over to liquid phase, thereby be particularly suitable for the flue-gas denitrification that main component is NO, removal efficiency is high, but because of the Fe in the absorbent
II(EDTA) easily by the O in the flue gas
2(volume content is generally 3-8%) oxidation and losing efficacy, and the complexed absorption agent is difficult to regeneration and recycle.And utilize the nitrogen oxide complexed absorption product of micro-reduction (to be mainly Fe
II(EDTA) NO, Fe
III(EDTA)), can solve the regeneration problem of complexed absorption agent well, so biological reducing coupling complexed absorption removes NO in the flue gas
xMethod is arisen at the historic moment.But because this method adopts free mixed bacteria, dominant bacteria density is little in the system, and is not strong to temperature and pH adaptive capacity, and be prone to cause assorted bacterium (like sulfate reducing bacteria etc.) to breed to make system's fluctuation of service, and system is low to the NO removal efficiency under high load capacity; Fe in the absorption liquid
II(EDTA) NO is to Fe
III(EDTA) reduction has very strong inhibitory action, and when carbon source is restricted nutrients, some bacterial classification Fe capable of using
II(EDTA) as electron donor, reduction Fe
II(EDTA) NO the time again with Fe
II(EDTA) be oxidized to Fe
III(EDTA).Thereby mixed microorganism can't satisfy the demand under the actual exhaust gas volumn to the rate of reduction of absorption liquid, particularly to Fe
III(EDTA) low rate of reduction makes Fe
III(EDTA) reduction becomes the rate determining step of whole system.Therefore, the quantity of dominant bacteria and performance in the how raising system reduce Fe
II(EDTA) NO is to Fe
III(EDTA) inhibitory action of reduction, the bacterial classification stable performance of keeping on top is to realize complexed absorption agent holomorphosis (promptly not producing secondary pollution), makes that system reaches efficiently, the key point of stable operation.
[summary of the invention]
Technical problem to be solved by this invention is to provide a kind of and does not produce secondary pollution and the high magnetic bio microballoon two-stage reductive coupling complexed absorption of purification efficiency removes NO in the flue gas
xTechnology.
The present invention solves the problems of the technologies described above through following technical scheme: a kind of magnetic bio microballoon two-stage reductive coupling complexed absorption removes NO in the flue gas
xTechnology, this technology may further comprise the steps:
(1) with the chitosan magnetic micro-sphere is Fe after fixation support will be tamed
II(EDTA) NO reduction bacterium, Fe
III(EDTA) after the immobilization of reduction bacterium difference, be filled in first order reducing/regenerating tower, second level reducing/regenerating tower respectively;
(2) contain Fe toward interior injection of the reservoir on absorption tower
II(EDTA) absorption liquid will contain NO afterwards
xSimulated flue gas feed in the absorption tower and contact NO with this absorption liquid
xWith the Fe in the absorption liquid
II(EDTA) complex reaction taking place is absorbed; Wherein absorption liquid includes basal medium, Fe
II(EDTA), carbon source, and electron donor;
(3) intensity of magnetization according to chitosan magnetic micro-sphere in first order reducing/regenerating tower, the second level reducing/regenerating tower applies corresponding current strength to first order reducing/regenerating tower, second level reducing/regenerating tower respectively; Afterwards with complexed absorption NO
xAfter absorption liquid earlier with first order reducing/regenerating tower in Fe
II(EDTA) NO reduction bacterium contact is with Fe
II(EDTA) NO is reduced to N
2, subsequently again with the Fe of second level reducing/regenerating tower
III(EDTA) reduction bacterium contact is with Fe
III(EDTA) be reduced to Fe
II(EDTA), make absorption liquid be able to regeneration.
Further, the component of basal medium: K described in the step (2)
2HPO
43H
2O 1000mg/L, KH
2PO
4625mg/L, Na
2SO
370mg/L, MgSO
4100mg/L, CaCl
22mg/L, MnSO
40.5mg/L, Na
2MoO
40.1mg/L, CuSO
45H
2O 0.1mg/L.
Further, carbon source described in the step (2) and electron donor are one or more in glucose, ethanol, the acetate.
Further, said simulated flue gas contains NO, reaches O
2
Further, said absorption tower is a packed absorber.
Magnetic bio microballoon two-stage reductive coupling complexed absorption of the present invention removes NO in the flue gas
xThe beneficial effect of technology be: through the movement velocity and the direction of externally-applied magnetic field control chitosan magnetic biological microsphere; Strengthened the process of mass transfer and heat transfer, can improve the density of system advantage bacterial classification, the bacterial classification stable performance of keeping on top; Overcome the substrate competition property inhibition problem between component in the absorption liquid; Improve biological reducing speed, realize not producing the purpose of secondary pollution, and have higher purification efficiency.
[description of drawings]
Combine embodiment that the present invention is further described with reference to the accompanying drawings.
Fig. 1 is a process chart of the present invention.
[specific embodiment]
1. enrichment of microorganism and domestication
(1) microbial enrichment
Get an amount of sewage treatment plant denitrification pond mud, leave standstill 24h after, the elimination supernatant takes off layer mud and basal medium and mixed in 1: 10 by volume and form mixed liquor, and this mixed liquor is placed culture dish, with NaNO
3(1000mg/L) as only nitrogen source, glucose (1000mg/L) carries out selective enrichment as sole carbon source to be cultivated, and uses N
2Drive water seal behind the oxygen, shaken cultivation under 40 ℃, the condition of 140r/min is treated in the culture dish
Lot of consumption and observed N
2After the generation,, collect thalline, be configured to bacterium liquid bacterium liquid centrifugation (centrifugal speed 5000r/min, centrifugation time 15min).
(2) microbial acclimation
Get the above-mentioned bacterium liquid that is configured to and be inoculated in the Fe that concentration is 2mmol/L respectively
II(EDTA) NO, Fe
III(EDTA) in the culture medium, bacterium liquid is 1: 10 with the culture volume ratio, and the pH value of culture medium all transfers to 6.5～7.0, and places shaken cultivation under 40 ℃, 140r/min condition; Every 6d changes once fresh culture medium and tames, and inoculation bacterium liquid is 1: 10 with fresh culture volume ratio, and is that gradient progressively increases Fe with 2mmol/L
II(EDTA) NO or Fe
III(EDTA) concentration in culture medium makes it finally reach 12mmol/L, always tame 30d after, can obtain Fe
II(EDTA) also original bacteria liquid and Fe of NO
III(EDTA) go back original bacteria liquid.
Basal medium is formed (unit: mg/L): K
2HPO
43H
2O 1000mg/L, KH
2PO
4625mg/L, Na
2SO
370mg/L, MgSO
4100mg/L, CaCl
22mg/L, MnSO
40.5mg/L, Na
2MoO
40.1mg/L, CuSO
45H
2O 0.1mg/L.The component of basal medium can be regulated, as long as can satisfy growth of microorganism.
2. the preparation of chitosan magnetic micro-sphere
In the preparation feedback device, be to add the ammonium ferric sulfate solution of 2% chitosan-acetic acid solution and 0.5mol/L at 3: 1 according to volume ratio, directly be warming up to 40 ℃ after stirring; The l ferrous ammonium sulfate solution (with the ammonium ferric sulfate solution equal-volume) that adds 0.5mol/L again; Under the 1200r/min high-speed stirred, evenly drip solution in NaOH solution to the preparation feedback device of 2mol/L become shiny black till, then constant temperature stirs 30min, ultrasonic agitation 30min down, stirs 20min again, stirs and carries out decompress filter after finishing; And use distilled water washing magnetic microsphere first product to filtrating to be neutrality; Freezing, in-80 ℃ of following vacuum freeze dryings, promptly obtain chitosan magnetic micro-sphere at last.
3. chitosan magnetic biological microsphere
(1) Fe
II(EDTA) immobilization of NO reduction bacterium:
Get above-mentioned Fe after domestication
II(EDTA) NO also original bacteria liquid in blake bottle, add chitosan magnetic micro-sphere and contain Fe
II(EDTA) basal medium of NO, control bacterial concentration are 0.2g/L (weight in wet base), and the chitosan magnetic micro-sphere dosage is 60g/L, Fe
II(EDTA) NO concentration is 10mmol/, as carbon source, feeds N with the glucose of 1000mg/L
2Seal after driving oxygen, putting into temperature is 40 ℃, and rotating speed is shaken cultivation 3d in the shaking table of 140r/min, and microorganism fully is immobilized on the chitosan magnetic micro-sphere.
(2) Fe
III(EDTA) immobilization of reduction bacterium:
Get the Fe after the domestication
III(EDTA) go back original bacteria liquid in blake bottle, add chitosan magnetic micro-sphere and contain Fe
III(EDTA) basal medium, control bacterial concentration are 0.2g/L (weight in wet base), and the chitosan magnetic micro-sphere dosage is 60g/L, Fe
III(EDTA) concentration is 10mmol/, with the glucose of 1000mg/L as carbon source, the NH of 1000mg/L
4Cl feeds N as nitrogenous source
2Seal after driving oxygen, putting into temperature is 40 ℃, and rotating speed is shaken cultivation 3d in the shaking table of 140r/min, and microorganism fully is immobilized on the chitosan magnetic micro-sphere.
4. technology purified treatment flue gas of the present invention
See also Fig. 1, the concrete steps of technology of the present invention are following: (1) has Fe with the immobilization for preparing
II(EDTA) chitosan magnetic of NO reduction bacterium little 100, and immobilization Fe is arranged
III(EDTA) chitosan magnetic micro-sphere 200 of reduction bacterium is filled in first order reducing/regenerating tower 3, second level reducing/regenerating tower 4 respectively; (2) contain Fe toward interior injection of the reservoir on absorption tower 1
II(EDTA) absorption liquid will contain NO afterwards
xSimulated flue gas feed in the absorption tower 1 and contact NO with this absorption liquid
xWith the Fe in the absorption liquid
II(EDTA) complex reaction taking place is absorbed; This absorption liquid mainly contains basal medium, Fe
II(EDTA), carbon source and electron donor; (3) according to chitosan magnetic micro-sphere 100, and the intensity of magnetization of chitosan magnetic micro-sphere 200 respectively first order reducing/regenerating tower 3, second level reducing/regenerating tower 4 are applied corresponding current strength; Particularly, apply current strength through 5 pairs of first order reducing/regeneratings of hot-wire coil group tower 3, second level reducing/regenerating tower 4; Afterwards with complexed absorption NO
xAfter absorption liquid through pump 2 be evacuated to make in the first order reducing/regenerating tower 3 its earlier with first order reducing/regenerating tower 3 in Fe
II(EDTA) NO reduction bacterium contact is with Fe
II(EDTA) NO is reduced to N
2Then the absorption liquid in the first order reducing/regenerating tower 3 is delivered to second level reducing/regenerating tower 4 and makes the Fe in itself and the second level reducing/regenerating tower 4
III(EDTA) reduction bacterium contact is with Fe
III(EDTA) be reduced to Fe
II(EDTA), make absorption liquid be able to regeneration.
Wherein, simulated flue gas contains NO, reaches O
2, and NO accounts for more than 90%; Packed absorber can be adopted in absorption tower 2; Can adopt in glucose, ethanol, the acetate one or more as carbon source and electron donor; And complexed absorption NO
xAfter the absorption liquid main component be Fe
II(EDTA) NO and Fe
III(EDTA).
Is example with glucose as carbon source and electron donor, and the biochemical reaction formula in the technology then of the present invention is:
Fe
II(EDTA)+NO → Fe
II(EDTA) NO---formula [1]
4Fe
II(EDTA)+O
2+ 4H
+→ 4Fe
III(EDTA)+2H
2O---formula [2]
Need to prove that formula [1], formula [2] all react in the absorption tower 1; Formula [3] reacts in the first order reducing/regenerating tower 3; Formula [4] reacts in the second level reducing/regenerating tower 4.
In addition, its component of the basal medium of being mentioned in the present invention is: K
2HPO
43H
2O 1000mg/L, KH
2PO
4625mg/L, Na
2SO
370mg/L, MgSO
4100mg/L, CaCl
22 mg/L, MnSO
40.5mg/L, Na
2MoO
40.1mg/L, CuSO
45H
2O 0.1mg/L.
In addition, in order better technology of the present invention to be set forth explanation, the applicant following several embodiment that given an example.
Embodiment 1
The immobilization for preparing there is Fe
II(EDTA) chitosan magnetic of NO reduction bacterium little 100, and immobilization Fe is arranged
III(EDTA) chitosan magnetic micro-sphere 200 of reduction bacterium is filled in respectively in first order reducing/regenerating tower 3, the second level reducing/regenerating tower 4; With 40mmol FeSO
47H
2O, 40mmol Na
4EDTA, 40mmol Fe
II(EDTA), 5g glucose, 5g NH
4Cl, 31g KH
2PO
4, 50g K
2HPO
4Be dissolved in distilled water, and add the 500ml basal medium and make 5L and contain Fe
II(EDTA) smoke absorption liquid, and in absorption liquid injection absorption tower 1 reservoir that makes, start-up system will contain 360mg/m
3NO, 2.5% (v/v) O
2, 15% (v/v) CO
2, 2500mg/m
3SO
2, all the other are N
2Simulated flue gas feed in the absorption tower 1 and carry out complexed absorption, air inflow is 1000mL/min; Apply the current strength of 3A respectively through 5 pairs of first order reducing/regeneratings of electric coil group tower 3, second level reducing/regenerating tower 4, afterwards with complexed absorption NO
xAfter absorption liquid through pump 2 be evacuated to make in the first order reducing/regenerating tower 3 its earlier with first order reducing/regenerating tower 3 in Fe
II(EDTA) NO reduction bacterium contact, the absorption liquid in the first order reducing/regenerating tower 3 flows into second level reducing/regenerating tower 4 and Fe subsequently
III(EDTA) reduction bacterium contact is with Fe
III(EDTA) be reduced to Fe
II(EDTA), make absorption liquid be able to regeneration, and the flow of absorption liquid in whole process be 156mL/min, treat that technology moves a period of time after stable continuously, detect the content that purifies NO in the flue gas of back, can know that the clearance of NO is 86%.
Embodiment 2
Present embodiment is compared with embodiment 1, and unique difference is: O in the simulated flue gas on feeding absorption tower 1
2Content change, particularly, this simulated flue gas contains 360mg/m
3NO, 5% (v/v) O
2, 15% (v/v) CO
2, 2500mg/m
3SO
2, all the other are N
2Detect the content that present embodiment purifies NO in the flue gas of back, can know that the clearance of NO is 82%.
Embodiment 3
Present embodiment is compared with embodiment 1, and unique difference is: O in the simulated flue gas on feeding absorption tower 1
2Content change, particularly, this simulated flue gas contains 360mg/m
3NO, 8% (v/v) O
2, 15% (v/v) CO
2, 2500mg/m
3SO
2, all the other are N
2Detect the content that present embodiment purifies NO in the flue gas of back, can know that the clearance of NO is 80%.
To sum up, the present invention has strengthened the process of mass transfer and heat transfer through the movement velocity and the direction of externally-applied magnetic field control chitosan magnetic micro-sphere; Can improve the density of system advantage bacterial classification; The bacterial classification stable performance of keeping on top overcomes the substrate competition property inhibition problem between component in the absorption liquid, improves biological reducing speed; Realize not producing the purpose of secondary pollution, and have higher purification efficiency.
Claims (5)
1. a magnetic bio microballoon two-stage reductive coupling complexed absorption removes NO in the flue gas
xTechnology is characterized in that: this technology may further comprise the steps:
(1) with the chitosan magnetic micro-sphere is Fe after fixation support will be tamed
II(EDTA) NO reduction bacterium, Fe
III(EDTA) after the immobilization of reduction bacterium difference, be filled in first order reducing/regenerating tower, second level reducing/regenerating tower respectively;
(2) contain Fe toward interior injection of the reservoir on absorption tower
II(EDTA) absorption liquid will contain NO afterwards
xSimulated flue gas feed in the absorption tower and contact NO with this absorption liquid
xWith the Fe in the absorption liquid
II(EDTA) complex reaction taking place is absorbed; Wherein absorption liquid contains basal medium, Fe
II(EDTA), carbon source, and electron donor;
(3) intensity of magnetization according to chitosan magnetic micro-sphere in first order reducing/regenerating tower, the second level reducing/regenerating tower applies corresponding current strength to first order reducing/regenerating tower, second level reducing/regenerating tower respectively; Afterwards with complexed absorption NO
xAfter absorption liquid earlier with first order reducing/regenerating tower in Fe
II(EDTA) NO reduction bacterium contact is with Fe
II(EDTA) NO is reduced to N
2, subsequently again with the Fe of second level reducing/regenerating tower
III(EDTA) reduction bacterium contact is with Fe
III(EDTA) be reduced to Fe
II(EDTA), make absorption liquid be able to regeneration.
2. remove NO in the flue gas according to the said magnetic bio microballoon of claim 1 two-stage reductive coupling complexed absorption
xTechnology, it is characterized in that: the component of basal medium: K described in the step (2)
2HPO
43H
2O1000mg/L, KH
2PO
4625mg/L, Na
2SO
370mg/L, MgSO
4100mg/L, CaCl
22mg/L, MnSO
40.5mg/L, Na
2MoO
40.1mg/L, CuSO
45H
2O 0.1mg/L.
3. remove NO in the flue gas according to the said magnetic bio microballoon of claim 1 two-stage reductive coupling complexed absorption
xTechnology, it is characterized in that: carbon source described in the step (2) and electron donor are one or more in glucose, ethanol, the acetate.
4. remove NO in the flue gas according to the said magnetic bio microballoon of claim 1 two-stage reductive coupling complexed absorption
xTechnology, it is characterized in that: said simulated flue gas contains NO, and O
2
5. remove NO in the flue gas according to the said magnetic bio microballoon of claim 1 two-stage reductive coupling complexed absorption
xTechnology, it is characterized in that: said absorption tower is a packed absorber.
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Cited By (6)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| CN103554389A (en) * | 2013-09-27 | 2014-02-05 | 华侨大学 | Preparation method of magnetic polymeric microsphere used for immobilized iron reducing bacteria |
| CN109173696A (en) * | 2018-09-19 | 2019-01-11 | 浙江工业大学 | A kind of magnetic field-intensification liquid phase scrubbing combines the method for biodegradable organic exhaust gas |
| CN109200789A (en) * | 2018-11-21 | 2019-01-15 | 安徽工业大学 | A kind of kiln gas low-temperature biological enzymatic reduction denitrification apparatus and method |
| CN110327761A (en) * | 2019-06-28 | 2019-10-15 | 苏州仕净环保科技股份有限公司 | The technique of NOx in a kind of removing flue gas |
| CN111389193A (en) * | 2020-01-14 | 2020-07-10 | 中国石油大学(华东) | Method for synchronously removing dissolved methane and NOx |
| CN114515501A (en) * | 2022-03-17 | 2022-05-20 | 哈尔滨工业大学 | Sulfur circulation and complexing agent regeneration-based complexing absorption NO synchronous denitrification method |
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Cited By (6)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| CN103554389A (en) * | 2013-09-27 | 2014-02-05 | 华侨大学 | Preparation method of magnetic polymeric microsphere used for immobilized iron reducing bacteria |
| CN109173696A (en) * | 2018-09-19 | 2019-01-11 | 浙江工业大学 | A kind of magnetic field-intensification liquid phase scrubbing combines the method for biodegradable organic exhaust gas |
| CN109200789A (en) * | 2018-11-21 | 2019-01-15 | 安徽工业大学 | A kind of kiln gas low-temperature biological enzymatic reduction denitrification apparatus and method |
| CN110327761A (en) * | 2019-06-28 | 2019-10-15 | 苏州仕净环保科技股份有限公司 | The technique of NOx in a kind of removing flue gas |
| CN111389193A (en) * | 2020-01-14 | 2020-07-10 | 中国石油大学(华东) | Method for synchronously removing dissolved methane and NOx |
| CN114515501A (en) * | 2022-03-17 | 2022-05-20 | 哈尔滨工业大学 | Sulfur circulation and complexing agent regeneration-based complexing absorption NO synchronous denitrification method |
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Application publication date: 20121226 |